We demonstrate the use of polymeric zwitterions, namely, poly(sulfobetaine methacrylate) (PSBMA), as solution-processable work function reducers for inverted organic electronic devices. A notable feature of PSBMA is orthogonal solubility relative to solvents typically employed in the processing of organic semiconductors. A strong permanent dipole moment on the sulfobetaine moiety was calculated by density functional theory. PSBMA interlayers reduced the work function of a broad range of electrodes [indium tin oxide (ITO), Au, Ag, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), Cu, Al, and even graphene] by over 1 eV. By employing an ultrathin interlayer of PSBMA, one can reduce the electron injection barrier between ITO and C70 by 0.67 eV. As a result, the device performance of OPVs with PSBMA interlayers are significantly improved, and enhanced electron injection is demonstrated in electron-only devices with ITO, PEDOT:PSS and graphene electrodes. This work makes available a new class of dipole-rich, counterion-free, pH insensitive interlayers for use as strong work function reducers for any electrode.